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Efficient hydrogenation of aliphatic amides to amines over vanadium-modified rhodium supported catalyst
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2021-08-05 , DOI: 10.1016/j.apcata.2021.118301
Alex Pennetier 1 , Willinton Y. Hernandez 1 , Bright T. Kusema 1 , Stéphane Streiff 1
Affiliation  

This work presents a highly efficient catalytic hydrogenation system developed for the selective transformation of tertiary N,N-dimethyldodecanamide and secondary azepan-2-one amides to the corresponding amines. Industrial hydrogenation catalysts Pd/Al2O3, Pt/Al2O3 and Rh/Al2O3 were modified with vanadium (V) or molybdenum (Mo) species as oxophilic centres. The modified catalysts were prepared by deposition of V or Mo precursor on supported catalysts via impregnation method. The catalysts were characterized by ICP-OES, XRD, XPS, H2-TPR, FTIR, CO-chemisorption, TEM, SEM-EDX and TGA. Modified Rh-V/Al2O3 catalyst displayed the best performance affording high yield and selectivity >95 % to the desired tertiary and secondary amines at moderate reaction conditions of T < 130 °C and PH2 < 50 bar. The strong synergistic interaction and proximity of hydrogenation Rh0 sites and oxophilic Vδ+ sites in the bimetallic Rh-V/Al2O3 catalyst were determined to be beneficial for the selective dissociation of Cdouble bondO bond of the carboxamides into the desired amines.



中文翻译:

在钒改性的铑负载催化剂上将脂肪族酰胺有效加氢为胺

这项工作提出了一种高效的催化氢化系统,用于将叔N,N-二甲基十二酰胺和仲 azepan-2-one 酰胺选择性转化为相应的胺。工业加氢催化剂Pd/Al 2 O 3、Pt/Al 2 O 3和Rh/Al 2 O 3用钒(V)或钼(Mo)物质作为亲氧中心改性。通过浸渍法在负载型催化剂上沉积 V 或 Mo 前驱体制备改性催化剂。通过ICP-OES、XRD、XPS、H 2 -TPR、FTIR、CO-化学吸附、TEM、SEM-EDX和TGA对催化剂进行了表征。改性 Rh-V/Al 2 O3催化剂显示出最佳性能,在 T < 130 °C 和 P H2 < 50 bar 的温和反应条件下,对所需的叔胺和仲胺提供了高产率和 >95% 的选择性。双金属Rh-V/Al 2 O 3催化剂中氢化Rh 0位点和亲氧性V δ+位点的强协同相互作用和接近性被确定有利于羧酰胺的CO 键选择性离解成所需的胺。双键

更新日期:2021-08-17
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